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Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase
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A Spectroscopic Study on Nitrogen Electrooxidation to Nitrate.

Tieliang Li1, Shuhe Han1, Yuting Wang1

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|March 13, 2023
PubMed
Summary
This summary is machine-generated.

Electrocatalytic nitrogen oxidation reaction (NOR) mechanism was elucidated using in situ spectroscopy and mass spectrometry. The study reveals NOR proceeds via an associative pathway, with nitrogen bond cleavage coupled to hydroxyl addition.

Keywords:
Artificial Nitrogen FixationN2 ElectrooxidationNitrateReaction Pathwayin Situ Characterizations

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Area of Science:

  • Electrochemistry
  • Catalysis
  • Surface Science

Background:

  • Electrocatalytic nitrogen oxidation reaction (NOR) is a promising alternative for nitrate production.
  • Understanding the NOR mechanism is crucial for optimizing the process, but remains poorly understood due to limited knowledge of reaction intermediates.

Purpose of the Study:

  • To investigate the mechanism of the electrocatalytic nitrogen oxidation reaction (NOR) over a rhodium (Rh) catalyst.
  • To identify key reaction intermediates and elucidate the NOR pathway.

Main Methods:

  • Electrochemical in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) was used to detect reaction intermediates.
  • Isotope-labeled online differential electrochemical mass spectrometry (DEMS) was employed to track reaction pathways.

Main Results:

  • Spectroscopic analysis identified key intermediates including asymmetric NO2- bending and NO3- vibrations.
  • Mass spectrometry with isotope labeling confirmed the formation of N2O and NO.
  • The results indicate an associative mechanism for NOR, involving distal approach.

Conclusions:

  • The nitrogen oxidation reaction (NOR) over a Rh catalyst follows an associative mechanism.
  • The strong N≡N bond in N2 is broken concurrently with hydroxyl addition to the distal nitrogen atom.